Hydrogen production via water electrocatalysis is limited by the sluggish anodic oxygen evolution reaction (OER) that requires a high overpotential. In response, a urea-assisted energy-saving alkaline hydrogen-production system has been investigated by replacing OER with a more oxidizable urea oxidation reaction (UOR). A bimetal heterostructure CoMn/CoMn 2 O 4 as a bifunctional catalyst is constructed in an alkaline system for both urea oxidation and hydrogen evolution reaction (HER). Based on the Schottky heterojunction structure, CoMn/CoMn 2 O 4 induces self-driven charge transfer at the interface, which facilitates the absorption of reactant molecules and the fracture of chemical bonds, therefore triggering the decomposition of water and urea. As a result, the heterostructured electrode exhibits ultralow potentials of −0.069 and 1.32 V (vs reversible hydrogen electrode) to reach 10 mA cm −2 for HER and UOR, respectively, in alkaline solution, and the full urea electrolysis driven by CoMn/CoMn 2 O 4 delivers 10 mA cm −2 at a relatively low potential of 1.51 V and performs stably for more than 15 h. This represents a novel strategy of Mott-Schottky hybrids in electrocatalysts and should inspire the development of sustainable energy conversion by combining hydrogen production and sewage treatment.
In article number 2000556, Chenglin Yan, Guozhen Shen, Xianfu Wang, and co‐workers present a bimetal Schottky heterojunction using an in‐situ electrochemical turning strategy. With the self‐driven charge transfer and redistribution at the interface, the developed catalyst with its built‐in electric field demonstrates excellent bifunctional catalysis for both urea oxidation and hydrogen evolution in alkaline systems.
Phase‐transition‐induced electronic structure and geometry‐modulation‐increased edge sites are of great importance for boosting the electrocatalytic activity of MoSe2 toward hydrogen evolution reaction (HER). However, little efforts have been made to improve the intrinsic activity on per‐catalytic site of MoSe2 for HER. In this work, the electrocatalytic HER activities of MoSe2 are extremely enhanced by simple incorporation of boron which can reasonably engineer the electron transfer from Mo atoms to the active sites including B and Se atoms. Compared with the pristine 1T MoSe2, the as‐opimized B‐1T MoSe2 nanosheets show a reduced overpotential of 180 mV at current density of 10 mA cm−2, a lowered Tafel slope of 50.6 mV dec−1, and increased turnover frequency under a constant overpotential. While the electrochemical surface area of the catalyst after B‐incorporation is decreased, the improved inherent activity on per‐catalytic site and facilitated HER kinetics are demonstrated. The results pave the way to reasonably engineer the electron transfer to the active sites in the catalysts by B‐doping to boost the intrinsic activity on per‐catalytic site for electrocatalytic HER.
Electrocatalytic water splitting into hydrogen and oxygen is a promising and competitive way to supply future sustainable and clean energy without carbon emissions, [1][2][3] which consists of two half reactions, namely, hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Among these two reactions, water oxidation is the rate-determining step due to the complex four-electron transfer process with sluggish kinetics that often requires a high overpotential to promote the reaction Tuning energy levels plays a crucial role in developing cost-effective, earth-abundant, and highly active oxygen evolution catalysts. However, to date, little attention has been paid to the effect of using heteroatomoccupied lattice sites on the energy level to engineer electrocatalytic activity. In order to explore heteroatom-engineered energy levels of spinel Co 3 O 4 for highly-effective oxygen electrocatalysts, herein Al atoms are directly introduced into the crystal lattice by occupying the Co 2+ ions in the tetrahedral sites and Co 3+ ions in the octahedral sites (denoted as Co 2+ Td and Co 3+ Oh , respectively). Experimental and theoretical simulations demonstrate that Al 3+ ions substituting Co 2+ Td and Co 3+ Oh active sites, especially Al 3+ ions occupying the Co 2+ Td sites, optimizes the adsorption, activation, and desorption features of intermediate species during oxygen evolution reaction (OER) processes. As a result, the optimized Co 1.75 Al 1.25 O 4 nanosheet exhibit unprecedented OER activity with an ultralow overpotential of 248 mV to deliver a current of 10 mA cm -2 , among the best Co-based OER electrocatalysts. This work should not only provide fundamental understanding of the effect of Al-occupied different Co sites in Co 3-x Al x O 4 composites on OER performance, but also inspire the design of low-cost, earth-abundant, and high-active electrocatalysts toward water oxidation. Water Oxidation
With the outbreak and widespread of the COVID-19 pandemic, large numbers of disposable face masks (DFMs) were abandoned in the environment. This study first investigated the sorption and desorption behaviors of four antibiotics (tetracycline (TC), ciprofloxacin (CIP), sulfamethoxazole (SMX), and triclosan (TCS)) on DFMs in the freshwater and seawater. It was found that the antibiotics in the freshwater exhibited relatively higher sorption and desorption capacities on the DFMs than those in the seawater. Here the antibiotics sorption processes were greatly related to their zwitterion species while the effect of salinity on the sorption processes was negligible. However, the desorption processes were jointly dominated by solution pH and salinity, with greater desorption capacities at lower pH values and salinity. Interestingly, we found that the distribution coefficient ( K d ) of TCS (0.3947 L/g) and SMX (0.0399 L/g) on DFMs was higher than those on some microplastics in freshwater systems. The sorption affinity of the antibiotics onto the DFMs followed the order of TCS > SMX > CIP > TC, which was positively correlated with octanol-water partition coefficient (log K ow ) of the antibiotics. Besides, the sorption processes of the antibiotics onto the DFMs were mainly predominated by film diffusion and partitioning mechanism. Overall, hydrophobic interaction regulated the antibiotics sorption processes. These findings would help to evaluate the environmental behavior of DFMs and to provide the analytical framework of their role in the transport of other pollutants.
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